Atomic Scale Crystal Field Mapping of Polar Vortices in Oxide Superlattices

Susarla, Sandhya; García-Fernández, Pablo; Ophus, Colin; Das, Sujit; Aguado-Puente, Pablo; McCarter, Margaret; Ercius, Peter; Martin, Lane W.; Ramesh, Ramamoorthy; Junquera, Javier

doi:10.1017/s1431927622009850

Title: Atomic Scale Crystal Field Mapping of Polar Vortices in Oxide Superlattices

Abstract

Polar vortices in oxide superlattices can be utilized as potential candidates for data storage applications due to their unique polarization topologies. The structure and dipole arrangement in polar vortices has been studied via X-ray scattering techniques, (scanning) transmission electron microscopy ((S)/TEM) and computational calculations. However, the fundamental correlation between the atomic structure and the electronic structure (which is manifested in the chemical bonding) has heretofore not been explored. Further, The hybridization between nominally empty $$\textit{d}$$ orbitals on the B-site with the occupied O 2$$\textit{p}$$ orbitals favors the condensation of a polar (ferroelectric) state in $$\textit{AB}$$O₃ perovskite oxides. The complex, continuously rotating local polarization texture of the vortices, in turn, can result in especially intricate $$\textit{d}$$- orbital interactions. Soft X-ray spectroscopy can probe these interactions at the transition metal $$\textit{L}$$-edge, but these techniques do not have the spatial resolution to resolve variations within one vortex (~5 nm region). Electron energy loss spectroscopy (EELS) in the STEM mode uses inelastically scattered electrons to probe the core-shell excitations (empty density of states) of transition metals at atomic resolution.

Authors:

Susarla, Sandhya ^[1]; García-Fernández, Pablo ^[2]; Ophus, Colin ^[3]; Das, Sujit ^[4]; Aguado-Puente, Pablo ^[5]; McCarter, Margaret ^[4]; Ercius, Peter ^[3]; Martin, Lane W. ^[4]; Ramesh, Ramamoorthy ^[1]; Junquera, Javier ^[2]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States)
Univ. of Cantabria, Santander, Cantabria (Spain)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Univ. of California, Berkeley, CA (United States)
CIC nanoGUNE, San Sebastián (Spain)

Publication Date:: Fri Jul 22 00:00:00 EDT 2022

Research Org.:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

OSTI Identifier:: 1896700

Grant/Contract Number:: AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Microscopy and Microanalysis

Additional Journal Information:: Journal Volume: 28; Journal Issue: S1; Journal ID: ISSN 1431-9276

Publisher:: Microscopy Society of America (MSA)

Country of Publication:: United States

Language:: English

Subject:: 74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats


                    Susarla, Sandhya, García-Fernández, Pablo, Ophus, Colin, Das, Sujit, Aguado-Puente, Pablo, McCarter, Margaret, Ercius, Peter, Martin, Lane W., Ramesh, Ramamoorthy, and Junquera, Javier. Atomic Scale Crystal Field Mapping of Polar Vortices in Oxide Superlattices.  United States: N. p., 2022. 
Web.  doi:10.1017/s1431927622009850.

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                    Susarla, Sandhya, García-Fernández, Pablo, Ophus, Colin, Das, Sujit, Aguado-Puente, Pablo, McCarter, Margaret, Ercius, Peter, Martin, Lane W., Ramesh, Ramamoorthy, & Junquera, Javier. Atomic Scale Crystal Field Mapping of Polar Vortices in Oxide Superlattices.  United States.  https://doi.org/10.1017/s1431927622009850

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                    Susarla, Sandhya, García-Fernández, Pablo, Ophus, Colin, Das, Sujit, Aguado-Puente, Pablo, McCarter, Margaret, Ercius, Peter, Martin, Lane W., Ramesh, Ramamoorthy, and Junquera, Javier. Fri .  
"Atomic Scale Crystal Field Mapping of Polar Vortices in Oxide Superlattices".  United States.  https://doi.org/10.1017/s1431927622009850.  https://www.osti.gov/servlets/purl/1896700.

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@article{osti_1896700,

  title        = {Atomic Scale Crystal Field Mapping of Polar Vortices in Oxide Superlattices},

  author       = {Susarla, Sandhya and García-Fernández, Pablo and Ophus, Colin and Das, Sujit and Aguado-Puente, Pablo and McCarter, Margaret and Ercius, Peter and Martin, Lane W. and Ramesh, Ramamoorthy and Junquera, Javier},

  abstractNote = {Polar vortices in oxide superlattices can be utilized as potential candidates for data storage applications due to their unique polarization topologies. The structure and dipole arrangement in polar vortices has been studied via X-ray scattering techniques, (scanning) transmission electron microscopy ((S)/TEM) and computational calculations. However, the fundamental correlation between the atomic structure and the electronic structure (which is manifested in the chemical bonding) has heretofore not been explored. Further, The hybridization between nominally empty $\textit{d}$ orbitals on the B-site with the occupied O 2$\textit{p}$ orbitals favors the condensation of a polar (ferroelectric) state in $\textit{AB}$O3 perovskite oxides. The complex, continuously rotating local polarization texture of the vortices, in turn, can result in especially intricate $\textit{d}$- orbital interactions. Soft X-ray spectroscopy can probe these interactions at the transition metal $\textit{L}$-edge, but these techniques do not have the spatial resolution to resolve variations within one vortex (~5 nm region). Electron energy loss spectroscopy (EELS) in the STEM mode uses inelastically scattered electrons to probe the core-shell excitations (empty density of states) of transition metals at atomic resolution.},

  doi          = {10.1017/s1431927622009850},

  journal      = {Microscopy and Microanalysis},

  number       = S1,

  volume       = 28,

  place        = {United States},

  year         = {Fri Jul 22 00:00:00 EDT 2022},

  month        = {Fri Jul 22 00:00:00 EDT 2022}

}

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